废弃聚烯烃的高值化学回收研究进展

doi:10.16085/j.issn.1000-6613.2023-0556

化工进展 ›› 2023, Vol. 42 ›› Issue (8): 3965-3978.DOI: 10.16085/j.issn.1000-6613.2023-0556

废弃聚烯烃的高值化学回收研究进展

常印龙¹^,²(), 周启民¹^,²(), 王青月¹^,²(), 王文俊¹^,², 李伯耿¹, 刘平伟¹^,²()

^1.化学工程联合国家重点实验室（浙江大学），浙江大学化学工程与生物工程学院，浙江杭州 310027
^2.浙江大学衢州研究院，浙江衢州 324000

收稿日期:2023-04-09 修回日期:2023-05-12 出版日期:2023-08-15 发布日期:2023-09-19
通讯作者: 王青月,刘平伟
作者简介:常印龙（2000—），男，硕士研究生，研究方向为聚烯烃的催化裂解。E-mail：ylchang@zju.edu.cn
周启民（1998—），男，博士研究生，研究方向为聚烯烃的催化裂解。E-mail：zhouqimin@zju.edu.cn。
基金资助:
国家自然科学基金重大项目(22293060);山西浙大新材料与化工研究院研发项目(2022SZ-TD003)

Research progress in high value chemical recycling of waste polyolefins

CHANG Yinlong¹^,²(), ZHOU Qimin¹^,²(), WANG Qingyue¹^,²(), WANG Wenjun¹^,², LI Bogeng¹, LIU Pingwei¹^,²()

^1.State Key Laboratory of Chemical Engineering at ZJU, College of Chemical and Biological Engineering, Zhejiang University, Hangzhou 310027, Zhejiang, China
^2.Institute of Zhejiang University-Quzhou, Quzhou 324000, Zhejiang, China

Received:2023-04-09 Revised:2023-05-12 Online:2023-08-15 Published:2023-09-19
Contact: WANG Qingyue, LIU Pingwei

摘要/Abstract

摘要：

占全球塑料产量一半以上的聚烯烃，由于其稳定碳氢链结构，极难降解，废弃后带来了严重的“白色”污染和“微塑料”问题。研究废弃聚烯烃的可控化学回收，实现其资源化和升级循环利用，具有重要的意义。本文重点总结了聚烯烃催化裂解的方法、特点及过程机理，包括催化热解、加氢裂化和氢解；梳理了高值裂解产物如芳烃、轻质烯烃、润滑油等的生成机制以及裂解过程中常用的催化剂种类及其催化构效关系；讨论和介绍了裂解反应以及高值产物生成的过程强化手段，包括基于反应器设计的反应过程强化、基于高效分离材料设计的分离过程强化等方面的研究进展。通过高效催化剂的设计及反应和分离过程强化技术的研究，有望实现废弃聚烯烃低温可控裂解及产物的高值化利用。

关键词: 废弃聚烯烃, 化学升级回收, 催化裂解, 高值化利用, 过程强化

Abstract:

Polyolefin plastics account for more than half of the world's plastics and have an extremely long natural degradation time due to their stable hydrocarbon chain structure. The accumulation of plastic waste leads to serious environmental disasters such as "white pollution" and "microplastics". It is of great importance to focus on the chemical up-recycling of polyolefin waste. This paper summarized the characteristics of catalytic recycling of polyolefins including catalytic pyrolysis, hydrocracking and hydrogenolysis. An overview of the mechanism of formation of value-added products (e.g., aromatics, light olefins and lubricants) commonly used catalysts, and the relationship between structure and activity of catalysts in the cracking process was presented. Meanwhile, process intensification methods for producing high-value products were introduced, including intensification of the reaction process based on reactor design and intensification of the separation process based on the design of efficient separation materials. It was expected that controllable low-temperature pyrolysis and high-value recovery of waste polyolefins can be achieved through the development of high-efficiency catalysts and research on intensification technologies in reaction and separation processes.

Key words: waste polyolefin, chemical upgrade recycling, catalytic cracking, high-value utilization, process intensification

中图分类号:

TQ325.1

常印龙, 周启民, 王青月, 王文俊, 李伯耿, 刘平伟. 废弃聚烯烃的高值化学回收研究进展[J]. 化工进展, 2023, 42(8): 3965-3978.

CHANG Yinlong, ZHOU Qimin, WANG Qingyue, WANG Wenjun, LI Bogeng, LIU Pingwei. Research progress in high value chemical recycling of waste polyolefins[J]. Chemical Industry and Engineering Progress, 2023, 42(8): 3965-3978.

图/表 9

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废弃聚烯烃的高值化学回收研究进展

Research progress in high value chemical recycling of waste polyolefins

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塑料	反应器类型	催化剂	塑料/催化剂（质量比）	温度/℃	产物（质量分数）/%				参考文献
塑料	反应器类型	催化剂	塑料/催化剂（质量比）	温度/℃	轻质烯烃	芳烃	C₅~C₁₂（不含芳烃）	C₁₂₊	参考文献
HDPE	锥形喷口床	HZSM-5	—	500	60	10（单环）	15（C₅~C₁₁）	1	[36]
HDPE	锥形喷口床	HZSM-5	30	500	58	—	—	—	[37]
HDPE	间歇反应器	HUSY	10	550	10.6	18	—	—	[38]
HDPE	微波辅助热解	HZSM-5	5	620	—	22	35.9	13	[39]
LDPE	微波辅助热解	HZSM-5	6.7	450	—	21.4	—	—	[40]
LDPE	固定床	B-HZSM-5	0.025	600	65.5	10.2	16.5（C₅~C₁₁）	5.5	[41]
PP	固定床	FCC	4	550	—	23.1	34.6（C₈~C₁₂）	14	[42]
PP	流化床	HUSY	0.4	430	—	1.12（BTX）	54.7（C₅~C₉）	—	[43]
PP+NS^①	固定床	HZSM-5	1	800	—	12.2	—	—	[44]
PS^②	间歇反应器	天然沸石	10	450	—	34.4	—	—	[45]
PE+PP	流化床	Ga-ZSM-5	—	550	15.9（C₂~C₃）	44	—	—	[46]

塑料	催化剂	温度/℃	氢气压力/MPa	时间/h	塑料/催化剂（质量比）	产物（质量分数）/%				参考文献
塑料	催化剂	温度/℃	氢气压力/MPa	时间/h	塑料/催化剂（质量比）	C₁~C₄	汽油	柴油	润滑油	参考文献
HDPE	Pt/STO	300	1.2	96	5	—	—	—	42	[74]
HDPE	Ru/C	220	2	1	2.4	—	—	—	31.6	[75]
LDPE	Ru/CeO₂	240	6	8	34	9.7	22	62	—	[16]
LDPE	Pt/WO₃/ZrO₂+Hβ	250	3	2	10	4	73	20	—	[76]
LDPE	Pt/W/β	250	3	1	40	30.3	63.6	—	—	[77]
PP	Pt/W/β	250	3	1	40	47.1	50.8	—	—	[77]
LLDPE^①	Pt/W/β	250	3	1	40	31.8	65	—	—	[77]
LLDPE	Ru/Nb₂O₅	300	3	2	10	—	47	32	—	[78]
PE+PP（热解蜡）	Ni/Hβ+ZSM-5	300	2	2	18.8	30.2	33.5	23.5	19	[79]

塑料	催化剂	温度/℃	氢气压力/MPa	时间/h	塑料/催化剂（质量比）	产物（质量分数）/%				参考文献
塑料	催化剂	温度/℃	氢气压力/MPa	时间/h	塑料/催化剂（质量比）	C₁~C₄	汽油	柴油	润滑油	参考文献
HDPE	Pt/STO	300	1.2	96	5	—	—	—	42	[74]
HDPE	Ru/C	220	2	1	2.4	—	—	—	31.6	[75]
LDPE	Ru/CeO₂	240	6	8	34	9.7	22	62	—	[16]
LDPE	Pt/WO₃/ZrO₂+Hβ	250	3	2	10	4	73	20	—	[76]
LDPE	Pt/W/β	250	3	1	40	30.3	63.6	—	—	[77]
PP	Pt/W/β	250	3	1	40	47.1	50.8	—	—	[77]
LLDPE^①	Pt/W/β	250	3	1	40	31.8	65	—	—	[77]
LLDPE	Ru/Nb₂O₅	300	3	2	10	—	47	32	—	[78]
PE+PP（热解蜡）	Ni/Hβ+ZSM-5	300	2	2	18.8	30.2	33.5	23.5	19	[79]